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Lamellar quasi-solid electrolyte with nanoconfined deep eutectic solvent for high-performance lithium battery

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Abstract

Electrolytes with high-efficiency lithium-ion transfer and reliable safety are of great importance for lithium battery. Although having superior ionic conductivity (10−3–10−2 S·cm−1), traditional liquid-state electrolytes always suffer from low lithium-ion transference number \(({t_{{\rm{L}}{{\rm{i}}^ + }}},\,\, < 0.4)\) and thus undesirable battery performances. Herein, the deep eutectic solvent (DES) is vacuum-filtered into the ∼ 1 nm interlayer channel of vermiculite (Vr) lamellar framework to fabricate a quasi-solid electrolyte (Vr-DES QSE). We demonstrate that the nanoconfinement effect of interlayer channel could facilitate the opening of solvation shell around lithium-ion. Meanwhile, the interaction from channel wall could inhibit the movement of anion. These enable high-efficiency lithium-ion transfer: 2.61 × 10−4 S·cm−1 at 25 °C. Importantly, the \({t_{{\rm{L}}{{\rm{i}}^ + }}}\) value reaches 0.63, which is 4.5 times of that of bulk DES, and much higher than most present liquid/quasi-solid electrolytes. In addition, Vr-DES QSE shows significantly improved interfacial stability with Li anode as compared with DES. The assembled Li symmetric cell can operate stably for 1000 h at 0.1 mA·cm−2. The lithium iron phosphate (LFP)∣Vr-DES QSE∣Li cell exhibits high capacity of 142.1 mAh·g−1 after 200 cycles at 25 °C and 0.5 C, with a capacity retention of 94.5%. The strategy of open solvation shell through nanoconfinement effect of lamellar framework may shed light on the development of advanced electrolytes.

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Acknowledgements

The authors would like to acknowledge financial support from National Natural Science Foundation of China (No. U2004199), Joint Foundation for Science and Technology Research & Development Plan of Henan Province (Nos. 222301420003 and 232301420038), China Postdoctoral Science Foundation (No. 2022TQ0293), and Key Science and Technology Project of Henan Province (No. 221100240200-06). Center for advanced analysis and computational science, Zhengzhou University is also highly acknowledged.

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  1. School of Chemical Engineering, Zhengzhou University, Zhengzhou, 450001, China

    Shiwei Liu, **g Wang, Keqi Wu, Zhirong Yang, Yan Dai, Junmei Zhang, Wenjia Wu & **gtao Wang

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  1. Shiwei Liu
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Correspondence to Zhirong Yang or Wenjia Wu.

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Liu, S., Wang, J., Wu, K. et al. Lamellar quasi-solid electrolyte with nanoconfined deep eutectic solvent for high-performance lithium battery. Nano Res. 17, 6176–6183 (2024). https://doi.org/10.1007/s12274-024-6620-7

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